Enhancing Compatibility of Two‐Step Tandem Catalytic Nitrate Reduction to Ammonia Over P‐Cu/Co(OH)₂

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 11, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach to realize ammonia generation and wastewater treatment. However, the transformation from NO − NH involves multiple proton‐coupled electron transfer processes by‐products 2 , H etc.), making high selectivity challenge. Herein, two‐phase nanoflower P‐Cu/Co(OH) electrocatalyst consisting of P‐Cu clusters P‐Co(OH) nanosheets designed match two‐step tandem process ) more compatible, avoiding excessive accumulation optimizing whole reaction. Focusing on initial 2e process, inhibited * desorption Cu sites in gives rise appropriate released electrolyte. Subsequently, exhibits superior capacity for trapping transforming desorbed during latter 6e due thermodynamic advantage contributions active hydrogen. In 1 m KOH + 0.1 leads yield rate 42.63 mg h cm Faradaic efficiency 97.04% at −0.4 V versus reversible hydrogen electrode. Such well‐matched achieves remarkable synthesis performance perspective catalytic reaction, offering novel guideline design RR electrocatalysts.

Language: Английский

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Homogeneously Mixed Cu–Co Bimetallic Catalyst Derived from Hydroxy Double Salt for Industrial-Level High-Rate Nitrate-to-Ammonia Electrosynthesis

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(40), P. 27417 - 27428

Published: Aug. 23, 2024

Electrocatalytic nitrate reduction reaction (NO

Language: Английский

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Effects of Ionic Interferents on Electrocatalytic Nitrate Reduction: Mechanistic Insight

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(29), P. 12823 - 12845

Published: July 2, 2024

Nitrate, a prevalent water pollutant, poses substantial public health concerns and environmental risks. Electrochemical reduction of nitrate (eNO

Language: Английский

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Photoelectrochemical Nitrate and Nitrite Reduction Using Cu₂O Photocathodes

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(5), P. 1993 - 1999

Published: April 4, 2024

Nitrate in wastewater streams causes eutrophication, and nitrate removal is of great importance for environmental protection. Electrochemical reduction has the advantage directly converting to benign or useful chemicals, but it typically requires a considerable overpotential. In this study, photoelectrochemical investigated using Cu2O photocathode, where photoexcited electrons conduction band inherently have an overpotential >1.6 V reduction. The photocathode found reduce nitrite selectively with high Faradaic efficiency (>85%). More importantly, as surface particularly catalytic reduction, on kinetically suppresses photocorrosion without need additional catalyst protection layers. addition examined compare effects kinetics photocurrent generation photocathodes.

Language: Английский

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Regulating the Electrochemical Nitrate Reduction Performance with Controllable Distribution of Unconventional Phase Copper on Alloy Nanostructures

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 6, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is emerging as a promising strategy for removal and ammonia (NH ) production using renewable electricity. Although great progresses have been achieved, the crystal phase effect of electrocatalysts on NO RR remains rarely explored. Here, epitaxial growth unconventional 2H Cu hexagonal close‐packed ( hcp IrNi template, resulting in formation three IrNiCu@Cu nanostructures, reported. IrNiCu@Cu‐20 shows superior catalytic performance, with NH Faradaic efficiency (FE) 86% at −0.1 (vs reversible hydrogen electrode [RHE]) yield rate 687.3 mmol g −1 h , far better than common face‐centered cubic Cu. In sharp contrast, IrNiCu@Cu‐30 IrNiCu@Cu‐50 covered by shell display high selectivity toward nitrite 2 − ), FE above 60% 0.1 RHE). Theoretical calculations demonstrated that has optimal electronic structures due to highest d‐band center strongest trend lowest energy barriers. The electroactivity originates from abundant low coordination sites surface, which guarantees fast electron transfer accelerate intermediate conversions. This work provides feasible tactic regulate product distribution engineering electrocatalysts.

Language: Английский

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Nanoflower‐Like CuPd/CuO Heterostructure for an Energy‐Output Electrocatalytic System Coupling Ammonia Electrosynthesis and Zinc‐Nitrate Battery

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 18, 2025

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) can effectively alleviate pollution and simultaneously realize ammonia electrosynthesis at room temperature. However, it remains a significant challenge for NO RR to achieve high Faradic efficiency in full concentration range. Herein, nanoflower‐like copper‐palladium alloy/CuO heterostructure (CuPd/CuO@NF) is successfully fabricated by the hydrothermal synthesis of CuO nanoflowers subsequent formation CuPd alloy. The as‐obtained CuPd/CuO@NF exhibits remarkable electrochemical performance − ‐N range from 20 1400 ppm, especially with conversion rate 97.8% NH selectivity 99.3% 94.2% yield 1.37 mmol h −1 cm −2 ppm. In‐situ Fourier transform infrared spectroscopy Raman spectra reveal that first catalyzes 2 , which rapidly reduced forming *NH, *NH OH intermediates. Density functional theory calculations suggest NHO route thermodynamically favorable. When applied zinc‐nitrate battery, demonstrates maximum power density 53.7 mW 99.9% 94.4%. This work offers valuable insights into design novel electrocatalysts batteries.

Language: Английский

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Phase‐Regulated Active Hydrogen Behavior on Molybdenum Disulfide for Electrochemical Nitrate‐to‐Ammonia Conversion

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(4)

Published: Dec. 8, 2023

Abstract Electrochemical reduction of nitrate waste is promising for environmental remediation and ammonia preparation. This process includes multiple hydrogenation steps, thus the active hydrogen behavior on surface catalyst crucial. The crystal phase referred to atomic arrangements in crystals has a great effect hydrogen, but influence still unclear. Herein, enzyme‐mimicking MoS 2 different phases (1T 2H) are used as models. Faradaic efficiency reaches ≈90 % over 1T‐MoS , obviously outperforming that 2H‐MoS (27.31 %). In situ Raman spectra theoretical calculations reveal produces more edge S sites at positive potential conducts an effortless pathway from instead energetically demanding steps (such *HNO *HNOH) performed .

Language: Английский

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Coordination and Architecture Regulation of Electrocatalysts for Sustainable Hydrogen Energy Conversion

Accounts of Materials Research, Journal Year: 2024, Volume and Issue: 5(2), P. 160 - 172

Published: Jan. 17, 2024

ConspectusWith the increasing concerns about energy and environmental crisis, hydrogen, with high density cleanliness, has been widely regarded as one ideal carrier for adjusting fossil fuel dependent system. In this context, extensive studies are focused on improving efficiency of sustainable hydrogen production, storage, utilization coupled renewable energy. And it can be realized in electrolysis cells cell devices. Several electrochemical reactions involved, such water splitting (hydrogen/oxygen evolution: HER/OER) electroreduction nitrogen/nitrate, carbon dioxide to NH3 HCOOH (NRR, NO3RR, CO2RR) oxygen reduction reaction (ORR) utilization. However, achieved conversion is still unsatisfactory due these intrinsically sluggish reactions, which spawned a revival research interests developing electrocatalysts activity, selectivity, durability. Therefore, various strategies have established construct effective electrocatalysts, coordination or architecture structure regulation, will determine intrinsic activity mass transport, respectively. Besides, combined progress characterization techniques theoretical studies, insightful understanding electrocatalytic sites mechanism also investigated, guiding rational design future electrocatalysts.In Account, we summarize our recent efforts exploring through regulation construction porous structures toward highly efficient conversion. First, an overview process presented reveal advantages challenges reactions. Then, introduced optimize enhance catalytic performance, tailoring particle size, valence state, crystal plane, defect engineering, substrate incorporation, structural reconstruction, etc. Additionally, illustrated study improvement performance via experimental calculations. Finally, brief outlook proposed address overcome catalysts.

Language: Английский

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Heterostructure Cu3P−Ni2P/CP catalyst assembled membrane electrode for high-efficiency electrocatalytic nitrate to ammonia

Nano Research, Journal Year: 2024, Volume and Issue: 17(6), P. 4872 - 4881

Published: Feb. 8, 2024

Language: Английский

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Complete Single-Pass Conversion of Dilute Nitrate to Ammonia Using Cu/Co(OH)₂ Tandem Electrocatalyst

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(8), P. 3849 - 3858

Published: July 15, 2024

Electrochemical nitrate reduction reaction (NO3RR) provides a promising route for the denitrification of wastewater and sustainable NH3 production but requires active selective electrocatalysts. Here, we demonstrate rigorous design tandem electrocatalyst efficient conversion NO3– to NH3. Based on screening components, catalyst coupling Cu Co(OH)2 with an optimal ratio architecture was developed promote balance activities sequential NO3RR steps different sites. Compared counterpart catalysts including Cu, Co(OH)2, Cu–Co alloy, Cu/Co(OH)2 separated phases showed much higher activity selectivity NH3, suggesting mechanism that involves NO2– solution transfer further Co-based When operated in flow cell, achieved 100% single-pass dilute at low overpotentials.

Language: Английский

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